Device for producing exothermic reactions between gases by contact with a solid catalyzer



ug. 9, E932., 1,870,665

DEVICE FOR PRODUCING EXOTHE'RMC REACTIONS BETWEEN GASES BY CONTACT WITHA SOLID CATALYZER Filed Nov. 7, 1929 5 Sheets-Sheet 1 BY f? ATTORNEYSyAug., 9, 1932. 1 E. AUDIBERT 1,870,665

DEVICE FOR PRODUCING EXOTHERMIC REACTIONS BETWEEN GASES BY CONTACT WITHA SOLID CATALYZER A Filed Nov. '7, 1929 3 SheeLS-Sheet 2 FLW INVENTOR BYe ATTORNEYS Aug. 9, 1932., E. AUDlBl-:RT 1,870,665 DEVICE FOR PRODUCINGEXOTHERMIC REACTIONS BETWEEN GASES BY CONTACT WITH A SOLID CATALYZERFiled Nov. 7, 1929 3 Sheets-Sheet 5 INVENTOR ATTORNEYS Patented Aug. 9,1932 UNITED STATES PATENTv OFFICE ETIENNE ADIIBERT, OF SENLIS, FRANCE,`ASSIGNOR TO SOCIETE NATIONALE DE RECHERCHES SUR LE TRAITEMENT DESCOMBUSTIBLES, OF SENLIS, FRANCE DEVICE FOR PRODUCING EXOTHERMICREACTIONS BETWEEN GASES BY CONTACT WITH A SOLID CATALYZER Applicationfiled November 7, 1929, Serial No. 405,495, and in France October 21,1929.

The present invention has foran object a device for producing exothermioreactions between gases by contact with a solid catalyz- `er, andparticularly for the synthetic manufacture either of ammonia gas ofmixtures of hydrogen and nitrogen, or of methanol or of any otherorganic compounds of mixtures of hydrogen and carbon monoxide.

A device in accordance with this invention, for producing exothermicreactions between gases by contact with a solid catalyzer, comprisesthree elements: a heat exchanger, a catalyzing tube and an apparatus forheating the fresh gaseous mixture, which .can be, according tocircumstances, placed 1n one, two or three distinct casings.

Two forms of construction of a device in accordance with this inventionare illustrated, by -way of example, in the accompanying drawings, inwhich:

Fig. 1 is a diagrammatic view of a form of construction in which thethree above mentioned elements are separated from each other.

Fig. 2 diagrammatically illustrates a second form of construction inwhich the catalyzing tube and the heating apparatus are connected in oneand the same casing.

Figs. 3 and 4 illustrate in vertical section and in a detailed manner,the essential elements of this second form of construction.

As shown in Fig. 1, the fresh gaseous mixture is admitted, through 1, 2,into the heat exchanger A, it circulates in the space 3 included betweenthe tubes 4, issues through 5, enters through 6 into the space 7included between the tubes 8 of the catalyzing apparatus B, issuesthrough 9 and is collected, after having passed through the heatingdevice 10, in the chamber 11, from which it passes into the tubes 8containing the Contact mass 8a;

the products of the reaction are fed, through 12 and 13, to the heatexchanger, from which they issue through 14. Y

l One of the features of the device forming the subject-matter of thepresent invention cbnsists in short-circuiting, on the one hand, theheat exchanger A, on the other hand, the intertubular space of thecatalyzing appara- 5 tus B, for instance by means:

Of a by-pass 15, 16, provided wth a cock 17, which puts the piping 1feedin the fresh mixture to the heat exchanger, in irect communicationwith the outlet piping 5 of this apparatus;

And of a by-pass 18-19, provided with a cock 20, which connects thepiping 6, feeding the gas to the intertubular space of the catalyzingapparatus, with the piping 9 feeding the gas to the heating apparatus.

Another mode of application of this principle consists, as shown by wayof example in'Fig. 2, in arranging on the pipings two identicalapparatus C and D which will be designated hereinafter under the name ofdistributors; these apparatus are shown in the form of cocks, the plugof which is provided with three channels and a notch, but they can beconstituted in any other manner capable of ensuring the followingoperation:

The distributor C serves to divide the stream of gaseous mixture sed asraw material into two branches, the relation in the outflows of whichcan be controlled at will by the said distributor C, only one of thesebranches passing through the heat exchanger A; with the arrangementshown in Fig. 2, for instance, a rotation of the plug in the cock body,in the direction of the arrow X,

has for effect to diminish the outiow through the heat exchanger' A, bycorrespondingly increasing the outflow of the stream which, through 1,21 and 22, is directlyconveyed to the distributor D.

Similarly, the distributor D serves to divide the gaseous stream issuingfrom the dis-v tributor C into two branches, the relation of theoutiiows of which can be controlled at will by this distributor D; oneof these branches is then directed towards the intertubular space 7 ofthe catalyzing apparatus B and subsequently towards the heating device10, the other branch being sent directly towards this heating device. Inthe 'case of Fig. 2, for instance, the first branch of the stream passesthrough 23, 24, 6, 7, 25 and 26, and the second branch through 23, 27and 9; a rotation of the cock plug in the direction of the arrow Yincreases the outiow of the 1 first branch at the expense of the outflowof the second branch.

The use of the two distributors which has just been described allows ofsuitably controlling the temperature of the contact mass and,consequentl on the one hand, of overcoming the deve opment of certainparasitic reactions of the main reaction as well as the prejudiciouseffects resulting, for the activity of a large number of catalyzers,from the fact that they are maintained at a too high temperature; on theother hand, of rendering the hourly production per litre of catalyticvolume independent from the Variations of activity of the contact mass.

In Fig. 2, both distributors are illustrated in the position whichcorresponds, for the tubes of the bundle, to the catalyzing apparatus Bwhen it is at its highestworking temperature; a rotation of the plugs ofthese distributors in the Adirection of the arrows X and Y allows ofmodifying this working temperature, owing to the putting in circulationin the intertubular s ace of a gaseous stream, the outflow of whic ,isadjustable, and the initial temperature of'which can moreover be variedbetween wide limits.

The catalyzing tube B, diagrammatically illustrated in Flg. 3, presentsive essential features, viz:

1. The contact mass is introduced in a series of vertical tubes 8,secured at both ends on two horizontal metal plates 28, 29; the upperplate 28 is secured, by screws or bolts, on a ledge 30 of the steelcasing 3l which supports the working pressure, whilst the lower late 29is free to move; the whole of the undle is thus suspended within thecasi-ng.

2. The contact mass is retained within the tubes 8 by a perforated plate32 rigid with a metal mem er 33 in the shape of a box assembled with thebottom plate by a fluidtight packing 34. The clamping of 33 on 29 isensured by clamping screws 35 carried by a member 36, which bears on aboss 37 of the bottom plate 29 through a. screwthreaded portion havinginterrupted threads, or in any other manner allowing the device to berapidly taken to pieces.

3. A chamber 10 is provided according to the axis of the catalyzingdevice and encloses the device for heating the fresh gaseous mixture;this heating device, diagrammatically indicated at 38 and suspended froman auxiliary plug 39, is completely independent from the remainder ofthe apparatus.

4. The gas contained in the intertubular space is brought in contactwith the device 38 by a member constituted by two coaxial tubes 40l and41, rigidly assembled together at their upper part on one and the sameannular cover; at the lower part, one of these tubes is permanentlysecured on the lower plate 29, Whilst the other can slide on a shoulder29a of this plate 29. On the other hand, these two tubes can freelyslide, at the upper part, through a circular orifice provided in theplate 28, the fluid-tightness of the joint being ensured by a plasticpacking 42.

5. Two co-axia-l tubes of small diameter, 43 and 44, secured on thelower plate 29, are inserted, with slight friction in correspondingbores of the lower plug 45 of the steel casing 4l, the fluid-tightnessof the assemblages being ensured by plastic packings 46 and 47 clamped,one by the plug 45, the other by a. stuffing-box 48.

The tube 43 serves for the direct introduction into the heating chamber10 of the fresh gaseous mixture admitted through the pipinv 9.

bThe tube 44 serves for evacuating outside the casing the products ofthe reaction which, when issuing from the bundle of tubes, are collectedin the metal member 33 and flow through an orifice 49 into the annularspace between 43 and 44.

The operation of the catalyzing device which has just been described isas follows: Both streams of fresh gaseous mixture separated by thedistributor D, enter the catalyzing apparatus, one through 6, the otherthrough 9. The gas introduced through 6 passes upwardly through theintertubular space 7, enters, through the orifices 25, into the annularspace comprised between the tubes 40 and 41, circulates downwardlybetween these tubes, and, through orifices 26, enters the heatingchamber 10, where it mixes with the gas admitted through 9. The mixturerises along the heating device 38 to the upper chamber 11, where itpasses into the tubes 8 containing the contact mass; it passesdownwardly through these tubes and is collected in the metal member 33,being finally evacuated through the orifice 49, the annular spacebetween 43 and 44, and the piping 13.

The characteristic properties of the apparatus thus devised are thefollowing:

a. The Huid-tightness of the device controlling the circulation of thegas is ensured by means of a small number of plastic packings, whichlatter have, moreover, a small diameter.-

b. The various elements of this device can, however, freely expand; thisallows, when choosing the metals used for constructing the saidelements, of not taking into account the values of the coeiiicients ofexpansion and to exclusively take into consideration the mechanical andchemical conditions to be satisfied.

c. The contact mass inserted in the tubes 8 of the bundle can be rapidlyevacuated; for that purpose, it Suiiices to loosen the screws 35, torelease the member 36 from the boss 37 by rotation according to afraction of a revolution, and to lower the members 36 and 33.

d. The heating device is completely independent from the device used forproducing catalysis and ensuring the circulation of the gas; thisallows, on the one hand, to use the most varied heating sources;electricity, gaseous or liquid fluid, internal combustion, etc.,

and, on the other hand, to replace the heating apparatus, by simplyunscrewing the plug 39,

without having to touch any other member.

e. The device for producing the catalysis and ensuring the circulationof the gases is in contact with the steel casing only at very fewpoints; this particularly facilitates the application, on the inner faceof the said cas'- ing, of coatings which maybe advantageously used forpreventing the gaseous mixture from coming in contact with this casing.

f. The assemblage and taking to pieces of thle catalyzing tube iseffected with great faci ity.

The heat exchanger A, illustrated in detail in Fig. 4, presents threeessential features, viz:

1. The vertical tubes 4 of the bundle constituting one of the essentialelements of this heat exchanger, are secured at their ends on twohorizontal metal plates 50 and 51; the

upper plate 50 is secured, by screws, on an inner ledge of the steelcasing which supports the working pressure, whilst the lower plate 51 isfree to move. The bundle of tubes is thus suspended with the casing.

2. The lower plate 51 is completed by a member 53, in the shape of abox, with which it is assembled by a fluid-tight packing 54.

3. Two pipes of small diameter, 55 and 56, are in communication with theexterior: the pipe 55 being secured on the member 53 while the interiorof this member 53 is in communication with the tubes 4 of the bundle.The other pipe 56 being secured on the upper plate 50 and incommunication with the intertubular space 3.

These two tubes pass through the lower plug 57 and the upper plug 58 ofthe casing, through orifices in which they can freely slide, thefluid-tightness of the joints being ensured by plastic packings 59 and60.

The operation of the apparatus which has just been described is asfollows; the frac- 50 tion of the fresh gaseous mixture directed by thedistributor C towards the heat exchanger, enters therein through thepiping 2,

circulates in .the intertubular space 3, and

issues through the tube 56 and the piping 5. 55 The products of thereaction coming from the catalyzing device enter the heat exchangerthrough the piping 13, circulate downwardly in the tubes 4, they arecollected in the hollow member 53 and issue through 55 and 14.

The characteristic feature of this heat exchanging apparatus resides inthe fact that the fluid-tightness of the device ensuring the circulationof the gases is obtained without hindering the free expansion of itselements. 55 Claims:

1. In a device for producing reactions between gases by 'contact with acatalyzer, the combination of a casing, a perforated plate secured inthe upper part of this casing, a plurality. of tubes secured in theholes of the said plate, a second perforated plate loosely placed in thelower ortion of the said casing, the lower ends o the tubes beingsecured in the holes of this second plate, a catalyzing material in thesaid tubes, a hollow member detachably secured under the said secondplate, this member having perforated portions extending under the saidtubes and adapted to support the said catalyzing material.

2. In a device for producing reactions between gases by contact with acatalyzer, the combination of a casing, a perforated plate secured inthe vupper part of this casing, a plurality oftubes secured in the holesof the said plate, a second perforated plate loosely placed in the lowerportion of the said casing, thelower ends of the tubes being secured inthe holes of this second plate, a. catalyzing material in the saidtubes, a hollow member detachably secured under the said second plate,this member having perforated portions extending under the said tubesand adapted to support the said catalyzing material, a plug in thebottom of the said casing, this plug presenting a vertical conduit wideat the top and narrow at the bottom, the second perforated plate havingtwo concentric tubular extensions downwardly directed and adapted toslide with slight friction respectively in the wide and narrow portionsof the said conduit, the said hollow member having an annular shape andsurrounding the outer tubular extension, this last tubular extension andthe said hollow member having registering orifices, and inlet and outletconduits respectively communicating with the said tubular extensions.

3. In a device for producing reactions between gases by contact with acatalyzer, the combination of a casing, a perforated plate secured inthe upper part of this casing, a plurality of tubes secured in the holesof the said plate, a second perforated plate loosely placed in the lowerportion of the said casing, the lower ends of the tubes being secured inthe holes of this second plate, a catalyzing material in the said tubes,a hollow member detachably secured under the said second plate, thismember having perforated portions extending under the said tubes andadapted t0 support the said catalyzin g material, two concentric sleevessecured at their lower part on the second perforated plate, the top ofthe Nouter sleeve being connected in a fluid-tight manner to the top ofthe inner sleeve and being adjusted with slight friction in an openingof the said upper perforated plate, the said sleeves having sideorifices, one near their upper end the other near their lower lil-3 end,and a heating device within the inner sleeve.

4. In a device for producing reactions bctween gases, a .heat exchangercomprising the combination of a casing, an upper perforated platesecured in the upper portion of the said casing, a plurality of tubessecured in the holes of the said upper plate, a lower perforated platcloosely placed in the lower part of the casing, the lower ends of thesaid tubes being secured in the holes of the said lower plate, a hollowmember secured under the said lower plate, perforated plugs secured inthe top and in the bottom of the said casing` tubesrespectively securedto the center of the upper tubular plate and to the center of the saidhollow member, these tubes being fitted with slight friction in theopenings of the said plugs, and conduits respectively leading to the topand to the bottom of the said casing for the admission and evacuation ofthe gases.

5. Device for exothcrmic reactions between gases by Contact with a solidcatalyzer, comprising a heat exchanger having two spaces separated in afluid-tight manner, a catalyzing apparatus having two chambers, aplurality of tubes connecting these chambers, a solid catalyzingmaterial in these tubes and a casing enclosing the said tubes, a heatingdevice, pipings for supplying the gases to be treated and leading to oneof the spaces of the heat exchanger, pipings between the said space ofthe exchanger and the casing of the catalyzing apparatus, between thiscasing and the heating device, between this .heating device and one ofthe chambers of the catalyzing apparatus, between the other chamber ofthe catal zing apparatus and the second space of t e heat exchanger, anda piping for the exhaust of the gases of the reaction, starting from thesecond space of the exchanger.

6. Device for exothermic reactions between gases by Contact with a solidcatalyzer, comprising a heat exchanger having two spaces separated in afluid-tight manner, a catalyzing apparatus having two chambers, aplurality of tubes connecting these chambers, a solid catalyzingmaterial in these tubes and a casing enclosing the said tubes, a heatingdevice, and pipings for supplying the gases to be treated and leading toone of the spaces of the heat exchanger, pipings between this space ofthe exchanger and the casing of the catalyzing apparatus, between thesaid casing and the heating device, between this heating device and oneof the chambers of the catalyzing apparatus, between the other chamberof the catalyzing apparatus and the second space of the heat exchanger,an exhaust piping for the gases of the reaction starting from the secondspace of the exchanger, a by-pass between the inlet and the outlet ofthe casing of the catalyzing appa-l ratus, and control means on theseby-passes for controllin the passage of the gases through these atter.

7. 1bn a device for reactions between gases by contact with a catalyzer,the combination of a casing, a perforated plate secured in the top ofthe said casing, a plurality of tubes secured in the holes of the saidplates, a second perforated plate loosely placed in the lower portion ofthe said casing, the lower ends of the tubes being secured in the holesof the second plate, a catalyzing material in the said tubes, and meansfor supporting the said catalyzing material in the said tubes.

8. In a device for producing reactions between gases by contact with acatalyst, the combination of a casing, a perforated plate secured in theupper part of this casing, a plurality of tubes secured in the holes ofthe said plate, a second perforated plate loosely placed in the lowerportion of the said casing, the lower ends of the tubes being securedyin the holes of this second plate, a catalyzing material in the saidtubes, a cylinder having perforated walls, secured axially to the secondplate, the rst plate having an orifice in which the said cylinder freelyslides, a fluid-tight packing between the said cylinder and the firstplate, and a heating device hung from the casing of the catalyzingapparatus and arranged in the axis of the cylin- In testimony whereof Ihave hereunto affixed my signature.

ETIENNE AUDIBERT.

